Conversion of Natural Gas to Liquid Form Using a Rotation/Separation System in a Chemical Reactor

ABSTRACT

A system and method are provided for the separation of hydrogen from natural gas feedstock to form hydrocarbon radicals. Aspects of the system include perpendicular magnetic and electric fields, a method of radical formation that separates hydrogen from the reaction process, and a separation method based on centrifugal forces and phase transitions. The gases rotate in the chamber due to the Lorentz force without any mechanical motion. Rotation separates gases and liquids by centrifugal force. The lighter species are collected from the mid region endpoint of the apparatus and fed back for further reaction. A new concept of controlled turbulence is introduced to mix various species. A novel magnetic field device is introduced comprised of two specially magnetized cylinders. A novel control of temperatures, pressures, electron densities and profiles by, RF, microwaves, UV and rotation frequency are possible especially when atomic, molecular, cyclotron resonances are taken into account. The electrodes can be coated with catalysts; the entire apparatus can be used as a new type of chemical reactor.

CROSS-REFERENCE TO RELATED APPLICATIONS

This application is a division of copending application Ser. No.14/592,676 filed Jan. 8, 2015, under 35 U.S.C. 120.

FIELD

This disclosure generally relates to a method and apparatus to produceliquid hydrocarbons from gaseous fuel feedstock in a continuousflow-through reaction system.

BACKGROUND

The supply of energy from natural gas is restricted by the inability toeconomically transport gaseous energy forms from the production point tothe point of distribution or use. It is vastly more desirable to haveliquid versus gaseous hydrocarbons to make the recovery and transport ofthe energy economically feasible. As such, natural gas produced as abyproduct of crude oil extraction from onshore or offshore oil wells isoften simply burned off or “flared” as waste or unusable gas instead ofbeing harvested. A simple, cost efficient method of converting naturalgas to a more energy-dense liquid form without expensive refrigerationis therefore required. Current methods for liquefying natural gasinclude the Fischer-Tropsch and related processes, as well asrefrigeration and condensation to form liquefied natural gas (LNG).However, each of these methods is economically limited. This disclosuredescribes a superior method of liquefying natural gas for transport anddistribution to increase the worldwide supply of this natural andinexpensive energy source. This method is based on basic principles inphysics and chemistry, confirmed by theory and experiments.

SUMMARY

Embodiments of the present disclosure relate to a system and methods toproduce liquid and solid hydrocarbons from gaseous hydrocarbon feedstockin a continuous, flow-through reaction system without the use of acatalyst. Elements of this system include improvements byelectromagnetic plasma technologies, rotation critical in separatinghydrogen from hydrocarbon radicals, a conversion of gaseous hydrocarbonfeedstock to liquid hydrocarbons through the enriching of the feedstockin free radicals, and a separation of liquid hydrocarbon products andhydrogen gas from reacted gaseous hydrocarbon feedstock in a rotatingsystem. One aspect of the high frequency of rotation is that chemicalbonds may be broken by high centrifugal force (effective gravitationalor g field). One embodiment of the apparatus produces an electric fieldand hence a current is generated in a radial direction within a magneticfield generated in an axial direction. The radial electric field andaxial magnetic field together produces an E×B force, which acts uponcharged particles with a force in the azimuth direction with respect tothe axis of the chamber. A key feature of this design is itsscalability, as permitted by the novel electromagnetic design withoutany moving mechanical parts. Provision is made to further separate theliquids by arrays of collectors with appropriate pressures andtemperatures to take each liquid state out in its unique molecular form.

Scalability of the apparatus and process is an important advantage ofthis invention. One aspect contributing to this scalability is the useof a novel magnetic field source as described within. Furthermore,consistent with the immediate goal of optimizing the conversion ofnatural gas to LNG or liquid form, the apparatus described below isdesigned to possess simple and reliable controls of temperatures andpressures at the location where conversion takes place, namely at theouter shroud. Therefore this invention describes a general device forthe conversion of molecules to the four forms of matter: solid, liquid,gas and plasma. A further feature of this apparatus is expected toenhance the rate or efficiency of any process occurring within theapparatus. This is the introduction of “controlled turbulence” throughthe imposition of changes in the driving electric fields, therebychanging the temporal behavior of the electromagnetic forces and theconsequent changes in the rate of rotation. This controlled turbulencewill change the degree of mixing among molecules at different radii. Theforegoing and other objects, features and advantages of the presentdisclosure will become more readily apparent from the following detaileddescription of exemplary embodiments as disclosed herein.

In addition to the rotation apparatus described, it is also possible toimplement the apparatus with a separate or integrated RF source, forexample a plasma torch. RF is used to produce RF bond resonance or an RFplasma; heating electrons instead of the whole mass. This can be tunedand controlled to facilitate the chemical reactions that areadvantageous to the production of the desired end product. The RF sourcecan be separately constructed and attached to the rotation apparatus toprovide an influx of desired radical chemical species or it may beintegrated with or within the rotation device. Optionally, a nanotipelectron emitter can be emplaced (in approximately the same locations asan RF source would logically be placed) to facilitate the formation ofradicals and drive the desired chemical reactions. The addition of waterto produce methanol during the aforesaid processes is also suggested.The addition of integrated optical and mass spectrometric diagnostics,for instance a residual gas analyzer, is an option to assist in identifyof chemical and physical species and to assist in the control of thereactions. The electron density and temperature can be controlleddigitally through manipulation of any or all of the devices or optionsmentioned. UV wavelength produced with RF can be controlled to produceradicals and avoid complete breakdown of molecules. A keydifferentiation of this apparatus and its suggested options is that ionsin the process stream drive ˜10⁶ times their mass of neutrals atrotation frequencies up to 100,000 RPS.

The element of temperature within the reaction chamber may be controlledby RF frequency or by cooling or heating the reaction chamber. Theelement of pressure can be controlled by the frequency of rotation byvarying the electric field, the magnetic field, or both. The apparatuscan be configured with various geometries of the outer electrode orvacuum sheath and provided with catalytic surfaces. In combination withthe control of other variables described, a novel chemical reactor forsolid, liquid and gas products is disclosed.

BRIEF DESCRIPTION OF THE DRAWINGS

The following drawings form part of the present specification and areincluded to further demonstrate certain aspects of the presentdisclosure. The disclosure may be better understood by reference to oneor more of these drawings in combination with the detailed descriptionof specific embodiments presented herein.

FIG. 1 illustrates an exemplary horizontal system for the reaction andrecovery of fuel stocks in accordance with one aspect of the invention.

FIG. 2 illustrates an exemplary system showing how an RF excitationsource can be integrated with the apparatus to increase the efficiencyof producing ions.

FIG. 3 is a flow chart of an exemplary method for the reaction andrecovery of liquid hydrocarbons by the present invention.

FIGS. 4A-4D are schematics of various embodiments of the axial magneticfield configuration, where the axial magnetic field is produced usingpermanent magnets or electromagnets, or alternatively by axialmagnetization of magnetizable inner and outer electrodes. The schematicsalso show the electrode surfaces, which can be modified for catalyticpromotion of desired chemical reactions.

FIG. 5A is a side view of an exemplary small chamber with a permanentmagnet.

FIG. 5B is a cross-sectional view of FIG. 5A.

FIG. 6A is a side view of an alternate small chamber embodiment.

FIG. 6B is a cross-sectional view of FIG. 6A including a heat exchanger.

FIG. 7 is a schematic diagram of a gas collection system embodiment.

FIG. 8 is a schematic diagram of a complete setup in accordance with anembodiment of the invention.

FIGS. 9 and 10 show exemplary embodiments of array collectors forcollecting various liquefied natural gas products in accordance with theinvention.

FIG. 11 is a schematic diagram showing the use of microwave cavities tocouple electromagnetic energy into the rotation chamber of the system.

DETAILED DESCRIPTION

Natural gas molecules, e.g. methane or CH₄, which are caused to forminto “radical” species such as CH₃, CH₂, CH₁, et cetera (referred togenerically as CH_(X)), will readily react to form longer chainhydrocarbons with other radical hydrocarbons. Pentane (C₅H₁₂) is thefirst liquid hydrocarbon at room temperature to be formed by this chainlengthening. Feedstock natural gas in combination with an electron donorspecies such as argon can be made to rotate if an electric current ispassed through them in the presence of a magnetic field. Due to theLorentz force, proper rotation is achieved without any mechanicalmotion. Rotation of the gas in the chamber causes the separation ofheavy chemical species from light species by centrifugal forces. Reactednatural gas undergoes carbon chain lengthening. This process leads toformation of pentane species, which are non-volatile and are separatedfrom lighter species by centrifugal force and also by precipitation.Lighter and volatile gas species are recirculated for re-ionization andreaction until the end product, pentane (liquid at room temperature), isremoved. In the process of lengthening the hydrocarbon feedstock gas,its links to hydrogen atoms must first be broken so that other carbonatoms can be attached to them. The released hydrogen gas is quicklyextracted from the apparatus to avoid reformation of the initialspecies. This released hydrogen gas is a desirable feedstock for cleanenergy production.

The figures below describe an exemplary apparatus. However, theapparatus may be modified or constructed differently to afford betterscalability or suitability to a given chemical reaction or physicalseparation. For instance, the anode and cathode can be reversed; theanode and cathode may also comprise the magnetic field device; the outerelectrode may comprise the outer shroud of the apparatus or may becontained within an additional outer shroud.

The components of the system shown in FIG. 1 are listed below:

1. Cooling water input (solid arrow denotes liquid flow)2. Methane/argon gas input/feed3. Central discharge rod (anode in)4. Central discharge rod insulation5. Cylindrical inner cylindrical anode electrode6. External discharge shell (outer cylindrical cathode electrode,double-walled capped cylinder filled with cooling fluid, 1)7. Unreacted gas (methane, argon) feedback line8. Region of forced rotation and plasma formation within chamber9. Hydrogen gas output to reservoir10. Heavy gas and liquid product (pentane) output to reservoir11. Region of vacuum within chamber12. Magnetic field array13. Power supply (5-500 VDC)

Referring to FIG. 1, the system is operated within a dual cylindricalmagnet or magnetic field array (12). An outer shroud or cylindricalshell (6), made from a material such as stainless steel, is placedwithin the central cavity of the magnet 12. This shroud is closed withrespective ports pumping out solution and feeding in solution. Withinthis shroud, an inner electrode (5) is placed which is electricallybiased with respect to the shroud wall. The apparatus is then placedwithin the magnetic field of the magnetic field array 12. The outercylindrical shell (6) is provided with double walls to provide for flowtherethrough of a cooling solution (1) from an inlet port to an outletport. This inlet/outlet cooling flow through the outer shell (6)provides temperature control with typical fluids from approximately 50′Cto as low as −180′C with for instance liquid nitrogen. The outer shell(6) also acts as an electrode (cathode, ground). The anode consists of acentral discharge rod (3), insulation (4) and an exposed cylindricalanode (5). The magnet 12 may be a superconducting or non-superconductingmagnet having a magnetic field in the axial direction and perpendicularto the radial DC field between the anode (i.e. electrode 5) and cathode(i.e. shell 6). An electrical current is provided by a power supply(13), preferably but not restricted to 5 to 500V DC. The feedstocknatural gas is mixed externally to a desired proportion with anionizable gas, such as for example argon (or similar easily ionizablegas) and is fed into inlet (2) of the cylindrical shell (6). When thefeedstock gas is subjected to the electric field within region (8), aplasma is formed and the dissociation of the feedstock gas into CH_(X)radicals and hydrogen atoms begins; where the hydrocarbon chain increasein length is enabled by the presence of radicals such as CH₃ or CH₂,provided the detached hydrogen atoms migrate to the central region ofthe cylinder shell 6, where they are extracted as hydrogen gas. In thesame region (8) rotation of the ionized gases occurs due to the radialelectric field and the perpendicular magnetic field. A vacuum may beimposed within the cylindrical shell (6) through the region (11). Thegases react as they move left to right through region (8), producinglonger carbon chain species and hydrogen gas at different radii in thecylinder. Due to the high rotational velocity, heavier gases and liquidare forced to the outside of the cylindrical shell. This allows liquidpentane to be collected at a larger radius through output (10) andhydrogen to be collected through output (9) at the inner radius.Unreacted hydrocarbon gases and argon are recycled through feedback line(7) at a smaller middle radius. Dissociation of species is promoted andprolonged in time by the rotational forces and electric fields(primarily DC but optionally augmented with AC disruptive pulses) withinthe shroud or shell 6.

Alternatively, a newly designed permanent magnet consisting of the anodeand cathode can be used to replace the external superconducting magnet(12) to facilitate scaling and portability of the instrument. The rolesof electrodes as anodes and cathodes can be reversed without loss ofgenerality.

It is also possible to use an interior surface of an outer cylinder,whether it is the outer electrode or the vacuum shroud, to assist inchemical reactions. The interior surface may be coated with a catalystto enhance specific chemical reactions in concert with manipulation ofliquid or gas phases at the surface through control of temperature orpressure by means described herein.

FIG. 2 illustrates the addition of an RF source at two example locationson the apparatus. An RF source can be added to the apparatus depicted inFIG. 1 to dissociate gaseous hydrocarbons more efficiently and morequickly produce the desired liquid end product. The RF source producesan oscillating electric field that imparts energy to electrons. Forexample, a 3 kW RF amplifier (14) is tuned through a variable capacitor(15) and radiated through an antenna apparatus (16). The antenna (16)can for example be placed in the proximity of either one or both of theareas depicted as hatched boxes. The electrons produced by the RF sourceand radiated by the antenna into the cylindrical shroud break the C—Hbonds, thereby dissociating the molecules. The components are listedbelow.

14. Power supply15. Frequency tuner

16. Antenna(e)

The RF source placed for example externally to the apparatus wouldprovide an influx of desired radical species to the rotation speciesthrough inlet (2), (7). Alternatively, the RF source could be placedinternally (for example in the area of the hatched box at the right-handside of the shroud 6). The locations given as examples for the RF sourcemight also be used to emplace nanotip emitters to provide an electronsource to produce desired radical species. Another configuration usingmicrowave cavities to couple electromagnetic energy directly into thesystem is shown in FIG. 11 where the cavities 1101 surround the mainrotating chamber 1102. This kind of coupling allows an efficientionization of the input neutral gas mixtures. Such electromagnetic wavescan be modulated to produce desirable resonances of chemical bonds.Additionally, other forms of energy may be used such as microwaveenergy, infrared energy, and laser energy.

Additional inlets or outlets (not shown) could provide for the influxof, for example, water to produce methanol. Additional outlets couldallow for more discriminating separation of chemical reaction products.

It is further pointed out that hydrocarbon liquids or methanol can berotated as well using the Lorentz force associated with a current in theconducting fluid. Liquids have the advantage that it is simple toproduce charges in the liquid, which do not recombine. The Lorentz forcewill rotate the liquid and separation can occur. All discussions hereinon gases on separation and chemical reactions can be applied to aliquid; gases and liquids are generally considered as fluids.

FIG. 3 is a flowchart of one example of a desired process in accordancewith the present disclosure, illustrating an exemplary method for theproduction and recovery of liquid hydrocarbons from natural gasfeedstocks. The general principle is the reactivity of natural gasradicals with each other. Once gases are decomposed into hydrogen andradicals (301), the radicals are reactive because one covalent bond isopen or “dangling” and ready to combine with another radical to form anew stable molecule. At 302, the electric and magnetic fields (Lorentzforce) produce rotation of the hydrocarbon plasma and a consequentcentrifugal force. At 303, H₂ forms and is separated from thehydrocarbon molecules by the rotation of the plasma. The remainingradicals react with each other to form longer chain hydrocarbons. At304, the longer chain hydrocarbon molecules in liquid form are collectedat room temperatures, and lighter (e.g. hydrogen) gases may be recycledthrough the system for repeated processing.

FIG. 4A is a conceptual schematic of a new method of producing an axialmagnetic field in the space between the inner electrode (5) and theouter shell (6) (functioning as an outer electrode), concentriccylindrical electrodes, as well as along the surfaces of the inner andouter electrodes. The axial magnetic field along the radial electricfield together provide the E×B force that acts to move charged particlesbetween the electrodes and at the electrode surfaces in an azimuthaldirection, with respect to the common, center axis of the concentriccylindrical electrodes.

In a first embodiment as shown in FIG. 4B, the axial magnetic field (“Bfield”) between the inner (5) and outer (6) electrodes is provided by anannular or a pair of external annular permanent magnets 12-B, which aremagnetized in the axial direction. The inner (5) and outer (6)electrodes are located between the pair of annular magnets, where theuse of annular magnets efficiently provides the axial magnetic fieldprimarily between the inner and outer electrodes and along theirsurfaces.

In a second embodiment as shown in FIG. 4C, an electromagnet, such as asuperconducting electromagnet 12-C, provides the axial magnetic fieldbetween the inner (5) and outer (6) electrodes and along their surfaces.Adjustable axial magnetic fields, whose intensity can be adjusted, areprovided by superconducting magnet 12-C.

A third embodiment, shown in FIG. 4D, allows the economic and efficientscalability of providing an axial magnetic field between the inner (5)and outer (6) concentric electrodes and along their surfaces. In thisthird embodiment the inner (5) and outer (6) electrodes are comprised ofa magnetizable material, which is magnetized in the same axialdirection. The permanently, axially magnetized inner (5) and outer (6)electrodes also provide axial magnetic field lines in the gap betweenthe inner and outer electrodes. The magnetizable material of the innerand outer electrodes can be magnetized in the same axial direction by anon-superconducting or superconducting electromagnet. By magnetizing theinner and outer cylindrical electrodes, the axial magnetic field B maybe introduced without either the additional use of a superconductingmagnet or use of an external pair of annular permanent magnets. Thisimprovement greatly decreases cost and increases the scalability andportability of the apparatus.

In addition to being used as the magnetic source, both the innerelectrode (5) and outer electrode (6) may have a catalytic coating onthe interior surface to assist in desired chemical reactions.

The magnetic array or superconducting magnet is used to generate amagnetic field in the axial direction z perpendicular to the radialdirection, while the electric field is generated by the power supply inthe radial direction. The current generated from the power supply in theradial plane perpendicular to the magnetic field in the axial planeinduces a rotational force about the z-axis. This force is called theLorentz force, represented by the following formula: F=J·B, where F isthe rotational force (Lorentz force), J is the current densityperpendicular to the B field and B is the magnitude of the magneticfield. The rotational force is dependent on the transfer of charges fromthe central electrode (5) to the wall of the outer shroud (6).

Using the system illustrated in FIGS. 1 and 2, extremely high rotationvelocities can be achieved that directly contribute to an extremely highseparation efficiency, as shown in the following equation:

${{q(r)} + 1} = {\exp\left( \frac{\omega^{2}r^{2}\Delta \; m}{2{kT}} \right)}$

wherein q is the separation factor, ω is the rotation rate, r is theradius, Δm is the species mass difference, k is the Boltzmann constantand T is the temperature. The equation shows that the separationefficiency depends exponentially on the square of the rotation velocity.

Rotation and current are the two main factors that contribute to theemergence of hydrocarbon radicals and hydrogen in atomic forms.Centrifugal forces, local heating by electrical current,micro-turbulence as well as molecular collisions contribute to theformation of desired chemical and atomic species being rotated.

A compact module can be designed using permanent magnets and transportedto needed locations for the processing natural gas. These modules forman array for series or parallel operation. In the case of seriesoperation, each outlet is sent forward for further purification. Asuccessive or tandem operation is equivalent to the purification insideone single unit of a larger diameter. The parallel operation allows fora larger throughput.

FIGS. 5A-5B, 6A-6B, 7 and 8 show various system implementations inaccordance with the present disclosure. In all embodiments as shown,cooling water comes into the chamber through an inlet and flows betweenthe double walls of the chamber to cool down the shroud. Two coolinglines connect a heat exchanger with the inner electrode. Hot water flowsout to the heat exchanger through an outlet, where heat is removed fromthe water. The cooled water is then run back to the inner electrode in acontinuous operating cycle, which enables sustained chemical reactionsto take place in the chamber.

A residual gas analyzer (RGA) provides accurate composition data of bothmethane and propane in accordance with the amount present in each of thegiven states post-discharge from the chamber. The amounts of methane andpropane along with the percentage that each of them represents in thetotal amount of natural gas converted are obtained from a UtilitiesLibrary Menu of the RGA software. RGAs are well known mass spectrometersin the art and as such further detailed description is not providedherein. Given the variable pressures and temperatures of the differentforms of gas within the chamber, those skilled in the art will recognizethat various known methods to determine them accurately can be used inaccordance with the invention.

In accordance with a further aspect of the invention, a gas collectionsystem contains cooling water tubes and pressure gauges. Since differentliquefied natural gas products can be produced under differenttemperature and pressure conditions, the pressure gauges and coolingwater tubes adjust the pressure and temperature in the reaction chamberto attain the conditions needed for each product.

FIGS. 9 and 10 illustrate exemplary array collectors that collectdifferent liquefied products in accordance with well-known phasediagrams showing the conditions under which various different gasproducts such as methane, butane, propane, ethane, etc. will becomeliquefied. By using different collectors in a coupled array, each ofwhich is coupled to a digital flow controller including temperature andpressure gauges that actuate valves for the collector tanks, differentconditions can be created to collect different liquefied products suchas methane, butane, propane, ethane, and hydrogen gas. As pressureincreases from P1 to P5 as shown, the pressure becomes increasinglyhigher to meet the liquefaction conditions for each gas.

While the example embodiments discussed fuels such as pentane, methane,propane and butane, all higher order liquids such as gasoline, jetfuels, and diesel fuels are contemplated by the present disclosure andwill be recognized as being included in the scope of the followingclaims.

What is claimed is:
 1. Apparatus for chemical conversion of natural gasto liquefied form, comprising: a chamber; a voltage supply forestablishing a voltage difference within said chamber; an energy sourceconfigured to ionize components in a feedstock natural gas mixtureintroduced into said chamber to produce a plasma; and a magnetic sourcefor generating a magnetic field in said chamber in a directionperpendicular to said voltage difference, said magnetic field causingsaid plasma to rotate within said chamber in a direction about an axisof said chamber so as to cause dissociation of natural gas in saidmixture into hydrocarbon radicals and reaction of said radicals toinduce chemical reactions between said hydrocarbon radicals to formhydrocarbon molecules having increased hydrocarbon chain length fromsaid radicals; wherein at least one liquefied natural gas product fromsaid rotating ionized natural gas mixture is extracted from saidchamber.
 2. Apparatus as set forth in claim 1, wherein said energysource comprises an RF energy source.
 3. Apparatus set forth in claim 1,wherein said energy source comprises a microwave energy source. 4.Apparatus as set forth in claim 1, wherein said energy source comprisesan infrared energy source.
 5. Apparatus as set forth in claim 1, whereinsaid energy source comprises a laser energy source.
 6. Apparatus as setforth in claim 1, wherein said feedstock natural gas mixture comprises amixture of natural gas with a readily ionizable background gas. 7.Apparatus as set forth in claim 6, wherein said readily ionizablebackground gas comprises argon.
 8. Apparatus as set forth in claim 1,wherein said magnetic source comprises a superconducting magnet. 9.Apparatus as set forth in claim 1, wherein said magnetic sourcecomprises a permanent magnet.
 10. Apparatus as set forth in claim 1,further comprising an array of collectors that each collects a differentliquefied natural gas product in accordance with phase transitionconditions for different liquefied products.